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The earliest signs of settlement in the area date back to the time of the Neanderthals, around 80,000 years ago.

Evidence of Roman occupation such as Roman currency and tools have also been found in and around the site. The name "Montségur" comes from Latinmons securus ("safe hill") which evolved into mont ségur in Occitan.

In the late 1204 the chateau was fortified to guard the southern frontier.

In the Middle Ages the Montségur region was ruled by the Counts of Toulouse, the Viscounts of Carcassonne and finally the Counts of Foix. In 1243–44, at the end of the Albigensian Crusade, the Cathars (a religious sect considered heretical by the Catholic Church) who had sought refuge at the Montségur fortress were besieged by 10,000 troops, in what is now known as the siege of Montségur. In March 1244, the Cathars finally surrendered and approximately 244 were burned en masse in a bonfire at the foot of the pog when they refused to renounce their faith. Some 25 actually took the ultimate Cathar vow of consolamentum perfecti in the two weeks before the final surrender. The Inquisitors kept faithful accounts and included the names of many, who are remembered every year on the anniversary of the massacre on March 16. These names are also displayed at the museum in the village of Montsegur.

English heavy metal band Iron Maiden have a song named "Montségur" on their album Dance of Death about the massacre of the Cathars.

The French guitarist, Pierre Bensusan, composed and performs the piece "Montségur."[1]

Richard Stanley, renowned filmmaker and director, has featured Montsegur and various aspects of the castle's history in two documentaries: The Secret Glory in 2001 and The Otherworld, in 2013. Both concern the neo-Cathar revival of the nineteen twenties and thirties, its ramifications in the present day and the mythic connections between Montségur and the Grail.[2]